Carbon welding on graphene skeleton for phase change composites with high thermal conductivity for solar-to-heat conversion

Advanced phase change materials (PCMs) with three-dimensional (3D) thermal conductive skeletons reveal the promising prospect in the thermal management of lithium battery. However, the high filler-to-filler interfacial thermal resistance (ITR) arising from the weak interfacial contact connection in 3D skeleton is still challenging. Herein, we demonstrate a “carbon welding” strategy for reducing the filler-to-filler ITR in 3D graphene skeleton by achieving the lattice connection between contact graphene. Typically, the ordered 3D graphene skeleton was constructed by unidirectionally ice template assembling graphene nanoplates (GNP) with the assistance of poly (amic acid) (PAA). Imidization and carbonization treatments were employed to weld the adjacent GNP in 3D skeleton. The similar lattice structure of carbonized polyimide (PI) and graphene can result in the significant reduction of phonon scattering and ITR at these contact areas. After impregnation with polyvinyl alcohol (PEG), the high-performance PCMs with high-efficient phonon transmission expressway were obtained. As expected, the prepared composites reveal the high thermal conductivities with a maximum value of 7.032 W m−1 K−1 at ~11.6 vol% GNP, which is more than two-fold than that of the composite with uncarbonized skeleton. Finite element simulation and nonlinear model analyses confirm that the reduced filler-to-filler ITR in skeleton is the main reason for the improving thermal conductivity. In addition, the presence of 3D graphene skeleton can effectively avoid the leakage during solid–liquid phase change, and significantly improve the shape stability of the PCMs. At the same time, the graphene skeleton can endow the PCM with an excellent solar-to-heat conversion performance, which ensure a wide range of application in actual environment.